Journal
CHEMBIOCHEM
Volume 22, Issue 8, Pages 1430-1439Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cbic.202000721
Keywords
carbohydrates; ionisation enhancers; LALDI-MS; mass spectrometry; pyrenes
Funding
- University of Leeds PhD studentship
- EPSRC Core Capability Grant [EP/K039202/1]
- Yorkshire Forward
- Northern Way Initiative
- EPSRC [EP/K039660/1, EP/M028127/1]
- EPSRC [EP/M028127/1, EP/K039660/1, EP/K039202/1] Funding Source: UKRI
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A series of pyrene-based LDI reagents (LALDI tags) have been developed for labeling and analyzing reducing carbohydrates in complex biological samples without the need for additional chemical derivatization or purification. The study demonstrates the potential of LALDI-MS for glycomics and diagnostics by direct detection of lactose in cow's milk.
Matrix-assisted laser desorption/ionisation mass spectrometry (MALDI-MS) is widely used for the analysis of biomolecules. Label-assisted laser desorption/ionisation mass spectrometry (LALDI-MS) is a matrix-free variant of MALDI-MS, in which only analytes covalently attached to a laser desorption/ionisation (LDI) enhancer are detected. LALDI-MS has shown promise in overcoming the limitations of MALDI-MS in terms of sample preparation and MS analysis. In this work, we have developed a series of pyrene-based LDI reagents (LALDI tags) that can be used for labelling and LALDI-MS analysis of reducing carbohydrates from complex (biological) samples without the need for additional chemical derivatisation or purification. We have systematically explored the suitability of four pyrene-based LDI enhancers and three aldehyde-reactive handles, optimised sample preparation, and demonstrated the use of LALDI tags for the detection of lactose. We have also exemplified the potential of LALDI tags for labelling carbohydrates in biological samples by direct detection of lactose in cow's milk. These results demonstrate that LALDI-MS is a promising technique for the analysis of reducing carbohydrates in biological samples, and pave the way for the development of LALDI-MS for glycomics and diagnostics.
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